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N u c l e a r E n g i n e e r i n g a n d T e c h n o l o g y 4 8 ( 2 0 1 6 ) 1 2 3 0 e1 2 3 6

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Nuclear Engineering and Technology


journal homepage: www.elsevier.com/locate/net

Original Article

Experimental Investigation of Clay Fly Ash Bricks


for Gamma-Ray Shielding

Harjinder Singh Mann a,*, Gurdarshan Singh Brar b,


Kulwinder Singh Mann c,d, and Gurmel Singh Mudahar a
a
Department of Physics, Punjabi University, Patiala 147002, India
b
Department of Higher Education, Additional Project Director, SCO 66-67, Sector 17 D, Chandigarh 160017, India
c
Department of Applied Sciences, I.K. Gujral Punjab Technical University, Jalandhar 144601, India
d
Department of Physics, D.A.V. College, Bathinda 151001, Punjab, India

article info abstract

Article history: This study aims to determine the effect of fly ash with a high replacing ratio of clay on the
Received 2 September 2015 radiation shielding properties of bricks. Some interaction parameters (mass attenuation
Received in revised form coefficients, half value layer, effective atomic number, effective electron density, and ab-
7 March 2016 sorption efficiency) of clay fly ash bricks were measured with a NaI(Tl) detector at
Accepted 1 April 2016 661.6 keV, 1,173.2 keV, and 1,332.5 keV. For the investigation of their shielding behavior, fly
Available online 21 April 2016 ash bricks were molded using an admixture to clay. A narrow beam transmission geometry
condition was used for the measurements. The measured values of these parameters were
Keywords: found in good agreement with the theoretical calculations. The elemental compositions of
Absorption Efficiency the clay fly ash bricks were analyzed by using an energy dispersive X-ray fluorescence
Clay Fly Ash Bricks spectrometer. At selected energies the values of the effective atomic numbers and effective
Half Value Layer electron densities showed a very modest variation with the composition of the fly ash. This
Mass Attenuation Coefficients seems to be due to the similarity of their elemental compositions. The obtained results
were also compared with concrete, in order to study the effect of fly ash content on the
radiation shielding properties of clay fly ash bricks. The clay fly ash bricks showed good
shielding properties for moderate energy gamma rays. Therefore, these bricks are feasible
and eco-friendly compared with traditional clay bricks used for construction.
Copyright © 2016, Published by Elsevier Korea LLC on behalf of Korean Nuclear Society. This
is an open access article under the CC BY-NC-ND license (http://creativecommons.org/
licenses/by-nc-nd/4.0/).

1. Introduction power plants, space research, medicine, and in agriculture.


For safe working conditions, biological radiation shields must
In recent years, due to the development of nuclear science and provide adequate protection for personnel at a reasonable
technology, the use of radioactive sources is increasing in cost. The mass attenuation coefficient provides a wide variety
different fields such as in nuclear research centers, nuclear of information about photon penetration and the energy

* Corresponding author.
E-mail address: maurharjinder@gmail.com (H.S. Mann).
http://dx.doi.org/10.1016/j.net.2016.04.001
1738-5733/Copyright © 2016, Published by Elsevier Korea LLC on behalf of Korean Nuclear Society. This is an open access article under
the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
N u c l e a r E n g i n e e r i n g a n d T e c h n o l o g y 4 8 ( 2 0 1 6 ) 1 2 3 0 e1 2 3 6 1231

deposition in biological shielding and other dosimetric mate-


rials. Lead and concrete are the conventional gamma-ray I ¼ I0 eðm=rÞrt (1)
shielding materials. It is necessary to look for cheap and
locally available innovative alternate shielding material for where I0 and I are the incident and transmitted intensity of
the rapid expansion of the nuclear industry and the extensive photons respectively, r is the density and t is the thickness of
applications of radioactive materials. The new material the sample, and m/r is the mass attenuation coefficient
should be cost effective, eco-friendly, and preferably utilize denoted by mm. The mass attenuation coefficient, for a com-
industrial wastes. Due to industrialization, the generation of pound or mixture is given by:
waste has increased several fold. One of these wastes is coal X
mm ¼ wi ðmm Þi (2)
fly ash, which can be used in brick formation due to its
pozzolanic nature. In recent years, several relevant studies for where wi and (mm)i are the weight fraction and the mass
the measurement of linear and mass attenuation coefficients attenuation coefficient of the ith constituent element
for different materials such as building materials [1e5], con- respectively.
cretes [6e8], cements [9,10], polymers [11], marble [12], and The effective atomic number (Zeff) of any compound con-
glasses [13,14] have been carried out. Clay is a naturally sisting of different elements is based on the determination of
occurring material composed of fine grain minerals, which the total attenuation cross section for gamma rays and it can
shows plasticity when moist and becomes hard when dried or be obtained by the relation:
fired. Clay has been used in the manufacturing of bricks since
sa
ancient times. The clay soils have better photon energy ab- Zeff ¼ (3)
se
sorption characteristics than other soils [15].
Fly ash is one of the most plentiful and versatile byprod- where sa and se represent the average atomic cross section
ucts of thermal power plants. It is an airborne material of and the average electronic cross section respectively. The
extremely fine spherical shaped particles. Nowadays, fly ash is average atomic cross section can be obtained from:
being used in the manufacturing of bricks, blocks, cement,
1 X
landfills, and in the construction of light-weight aggregates. sa ¼ fi Ai ðmm Þi (4)
NA i
Fly ash can also be used as a radiation shielding material for
gamma rays after it is compacted to a high degree [16]. where mm is the total number of mass attenuation coefficients,
Therefore, research on the use of waste products will help to N is the Avogadro's number, Ai and wi are the atomic weights
solve many environmental problems. The effect of grain size and the fractional weights of the measured samples
and voids in various soil samples has been found to increase respectively.
the mass attenuation coefficient with the decrease of grain Similarly, the electronic cross section is given by:
size of these samples [17]. One of the possible ways to take
1 X fi Ai
advantage of the fine particle size of clay and the pozzolanic se ¼ ðm Þ (5)
NA i Zi m i
properties of fly ash is to prepare compacted bricks by the
incorporation of fly ash in clay at an optimum water content. The effective electron density (number of electrons per
Fly ash alone has insufficient plasticity to produce bricks unit mass) is given by:
strong enough to survive handling and drying, so binder clay   X
has to be added. The finer particles of fly ash will fill the pores m=r Zeff
Ne ¼ ¼ NA ni (6)
to reduce the void ratio and increase the strength of the bricks. se M i
The aim of this study was to explore the possibilities of the
The HVL (the thickness of radiation shielding material
utilization of fly ash, which was done by collecting fly ash and
needed to reduce the incident intensity of the gamma ray to
then compacting it with locally available clay in the form of
its half) can be calculated from the linear attenuation coeffi-
clay fly ash bricks to design and test it as a gamma-ray shield
cient m as:
in a cost effective way. However, to our knowledge, no studies
related to radiation parameters of fly ash mixed with clay in 0:693
HVL ¼ (7)
high volumes are available. These bricks exhibit good me- m
chanical properties such as high strength and durability.
However, in the present work, an attempt has been made to
measure gamma ray interaction parameters such as mass and
linear attenuation coefficients, half value layer (HVL), effective 2. Materials and methods
atomic number, and electron density for clay fly ash bricks
mixed in different proportions. To assess the shielding effec- The fly ash used in this study was collected from electrostatic
tiveness of the clay fly ash bricks, the absorption efficiency of precipitators of the Thermal Power Station Ropar, Punjab,
bricks for gamma rays was determined. India. The fly ash confirms the properties according to Indian
Standard: 3812 [18]. Locally available clay soil was used to
augment the cementitious properties of the fly ash. The
1.1. Theory semiquantification elemental analysis to identify the weight
percentage of major and minor elements present in the
A collimated beam of mono energetic gamma rays is attenu- samples was done using the OXFORD INCAx-act model (OX-
ated in the matter, according to the LamberteBeer law: FORD instruments) Energy Dispersive X-ray spectrometer
1232 N u c l e a r E n g i n e e r i n g a n d T e c h n o l o g y 4 8 ( 2 0 1 6 ) 1 2 3 0 e1 2 3 6

Table 1 e Elemental composition of fly ash, clay, and the mixtures.


Brick sample Density (g/cm3) Elemental weight (%)
O Al Si K Ca Fe Cu Zn
Fly ash 1.160 0.463 0.138 0.267 0.013 0.010 0.057 0.025 0.027
Clay 1.780 0.502 0.087 0.268 0.024 e 0.120 e e
CF10 1.730 0.498 0.092 0.267 0.023 0.001 0.113 0.002 0.003
CF20 1.610 0.493 0.097 0.267 0.022 0.002 0.107 0.005 0.005
CF30 1.600 0.490 0.102 0.267 0.021 0.003 0.101 0.007 0.008
CF40 1.560 0.486 0.107 0.267 0.020 0.004 0.095 0.010 0.011
CF50 1.540 0.482 0.112 0.267 0.019 0.005 0.088 0.012 0.013

CF10, 10% fly ash content; CF20, 20% fly ash content; CF30, 30% fly ash content; CF40, 40% fly ash content; CF50, 50% fly ash content.

available at Thapar University, Patiala. X-ray fluorescence is a porosity means higher density and better radiation attenua-
strong analytical tool used widely for determining element tion performance. The degree of compaction influences the
composition in an unknown sample, due to its nondestructive compressibility, stiffness, and compressive strength of the
properties and accuracy. This gives it an advantage over other bricks, to meet the required shielding characteristics.
techniques. The weight percentages of elements present in
the samples of clay and fly ash are given in Table 1. 2.2. Experimental set-up

2.1. Preparation of samples The mass attenuation measurements of the prepared samples
were performed using narrow beam gamma-ray transmission
The collected samples of fly ash and clay were mixed in geometry. The experiment set-up of standard transmission
different proportions in an attempt to find the strongest, most geometry used in the present study is shown in Fig. 1. The
economical mix. Additive clay was chosen to improve the samples were irradiated by photons emitted from 137Cs
plasticity indices of mixture. The clay fly ash bricks were (661.6 keV) and 60Co (1,173.2 keV and 1,332.5 keV) procured
prepared with fly ash contents of 10%, 20%, 30%, 40%, and 50% from Board of Radiation and Isotope Technology, Navi Mum-
and named CF10, CF20, CF30, CF40, and CF50, respectively. bai, India. The source was enclosed in a lead container with
When the proportion of fly ash in bricks was more than 50% by one face aperture of 6 mm, placed behind the source colli-
weight, then it was difficult to cast the bricks [19]. The samples mator. Two collimators with apertures of 4 mm and 2.8 mm
were weighed accurately using an electronic balance with an were placed with their front faces at a distance of 200 mm and
accuracy of 0.01 g and mixed thoroughly by adding the 550 mm from the source, respectively.
appropriate amount of distilled water. The mixture prepared The incident and transmitted gamma-ray intensities were
earlier was poured into the cubic clean casting mold, filling determined for a fixed preset time using the 300  300 Na(Tl)
one third at a time. During packing, the mixture was com- detector (CANBERRA, PMT base model (CANBERRA Industries);
pacted by applying equal blows in a uniform manner over the 802) having an energy resolution of 7.5% at 661.6 keV for a
surface to remove air for the densification of bricks. A trowel gamma ray from Cs-137. NaI crystal was integrally coupled to
was used to even out the surface. The high density of the a photomultiplier tube. The detector was shielded by a cylin-
compacted samples led to the reduction of porosity. Less drical lead shielding of approximately 8 cm thickness, which

Fig. 1 e Experimental set-up of standard transmission geometry. H.V., half value; MCA, multichannel analyzer; Pre-amp,
preamplifier.
N u c l e a r E n g i n e e r i n g a n d T e c h n o l o g y 4 8 ( 2 0 1 6 ) 1 2 3 0 e1 2 3 6 1233

Table 2 e Mass attenuation coefficients of clay fly ash bricks and concrete [2].
Samples 661.6 keV 1173.2 keV 1332.5 keV
Experimental Theoretical Experimental Theoretical Experimental Theoretical
Clay 0.0778 ± 0.0018 0.0766 0.0580 ± 0.0012 0.0582 0.0542 ± 0.0019 0.0546
CF10 0.0757 ± 0.0015 0.0766 0.0589 ± 0.0014 0.0582 0.0551 ± 0.0023 0.0546
CF20 0.0789 ± 0.0016 0.0766 0.0595 ± 0.0017 0.0582 0.0559 ± 0.0019 0.0546
CF30 0.0779 ± 0.0019 0.0765 0.0569 ± 0.0015 0.0581 0.0553 ± 0.0021 0.0546
CF40 0.0774 ± 0.0018 0.0765 0.0571 ± 0.0018 0.0581 0.0536 ± 0.0019 0.0546
CF50 0.0762 ± 0.0017 0.0765 0.0566 ± 0.0019 0.0581 0.0529 ± 0.0017 0.0546
Concrete [2] 0.073 ± 0.002 e 0.066 ± 0.001 e 0.060 ± 0.001 e

CF10, 10% fly ash content; CF20, 20% fly ash content; CF30, 30% fly ash content; CF40, 40% fly ash content; CF50, 50% fly ash content.

was also lined on the inside with brass and aluminum sheets The total experimental uncertainty of the measured mass
to stop the fluorescence X rays (approx. 75 keV) of lead from attenuation coefficients depends on the uncertainties of the
reaching the detector. The sample was positioned on the evaluation of peak areas of incident (I0) and transmitted
symmetry axis of the detector. The stability of the experi- intensities(I), thickness (t), and density (r) measurements and
mental set-up was tested using aluminum as a reference it can be calculated using the propagation of error formula:
absorber at 661.6 keV. The amplified signal from the detector sffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
   2  2  2  2ffi
was then fed to the multichannel analyzer, which converted m 1 DI0 DI I0 Dt
D ¼ þ þ ln (8)
the analog signal into a digital number through an analog to r rt I0 I I t
digital converter. The pulse height was recorded with a
where DI0, DI, and Dt are the errors in the intensities I0 and I,
computerized 2K multichannel analyzer plug-in card. While
and thickness t of the sample, respectively. The estimated
taking readings, a sufficient number of counts were collected
error in the experimental measurement was approximate 4%.
under the photo peak to limit the statistical error to < 0.5%.
These uncertainties are mainly due to counting statistics, the
The background counts, recorded at the same time, were
thickness and density measurements, the evaluation of peak
subtracted from each spectrum. The measurement of gamma-
areas, and deviations from narrow beam geometry in source-
ray attenuation counts at every energy was repeated a mini-
detector arrangements.
mum of three times before and after the sample was intro-
duced and the average value was used in calculations. The
laboratory temperature was kept at approximately 20 ± 1 C. 3. Results
The criterion mt < 1, where t is the thickness of the sample, was
used in order to minimize the number of multiple scattered The major, minor, and trace element levels in clay and fly ash
photons reaching the detector [20,21]. The whole apparatus have been determined using an energy dispersive X-ray fluo-
was also placed at a suitable distance from the walls of the rescence spectrometer. These values are then used to calculate
room so as to avoid the contribution of scattered photons from the total mass attenuation coefficients in the wide photon
the wall. energy range from 1 keV to 100 GeV. The experimental values

Fig. 2 e Variation of mass attenuation coefficient with Fig. 3 e Variation of linear attenuation coefficient with
incident photon energy. CF10, 10% fly ash content; CF20, incident energy for different clay fly ash bricks and
20% fly ash content; CF30, 30% fly ash content; CF40, 40% concrete. CF10, 10% fly ash content; CF20, 20% fly ash
fly ash content; CF50, 50% fly ash content; Exp., content; CF30, 30% fly ash content; CF40, 40% fly ash
experimental; Th., theoretical. content; CF50, 50% fly ash content.
1234 N u c l e a r E n g i n e e r i n g a n d T e c h n o l o g y 4 8 ( 2 0 1 6 ) 1 2 3 0 e1 2 3 6

agreement for all studied compositions. There is no large


variation between mass attenuation coefficient values at the
energy region (661.6 keV, 1,173.2 keV, and 1,332.5 keV), where
the Compton Effect is dominant, having linear Z dependence.
The mass attenuation coefficient is almost the same for all
chosen clay fly ash brick samples due to the similarity of
elemental compositions in each sample. Also, it is indepen-
dent of the density of the target material, but depends upon
the chemical composition of the material. The constancy of mm
for the chosen samples is in line with the theoretical findings
of Mudahar et al. [24], in which they reported that in the en-
ergy region 300 keV to 3 MeV, the variations in total mm for low
Z materials are negligible.
Fig. 3 shows the comparison of total linear attenuation co-
efficient (m) values for the mixture of clay fly ash bricks with
another shielding material common in the literature: concrete
[2]. The results showed an inverse relationship between the m
Fig. 4 e Variation of half value layer with fly ash content in
values and the energy E. At low energies, the linear attenuation
bricks. CF10, 10% fly ash content; CF20, 20% fly ash content;
coefficient decreases sharply due to the dominance of photo-
CF30, 30% fly ash content; CF40, 40% fly ash content; CF50,
electric effect; whereas at 1,173 keV and 1,332 keV, Compton
50% fly ash content.
scattering and pair production phenomena are dominant [8,25].
Also, the m values decrease with an increase in the percentage of
low density fly ash in the samples. By comparison with con-
of mass attenuation coefficients for concrete and clay fly ash crete, it can be noticed that for all clay fly ash brick samples, the
brick samples, mixed with different percentages by weight linear attenuation coefficients are less than those of concrete.
(10%, 20%, 30%, 40%, and 50%) of fly ash, are enlisted in Table 2 Therefore, for an improved shielding effectiveness, a larger
with the theoretical values calculated using the WinXCom thickness of the clay fly ash brick would be required.
computer program (WinXcom is Windows Version by L. Ger- The effectiveness of gamma ray shielding is described in
ward, Technical University of Denmark, DK-2800 Lyngby, terms of the HVL of the clay fly ash bricks and concrete as
Capital Region, Denmark) [22] initially developed as XCOM [23]. shown in Fig. 4. The HVL is the thickness at which an absorber
Fig. 2 shows that the experimental and theoretical values will reduce the radiation to half. The lower the value of HVL,
of the total mass attenuation coefficients are clearly in good the better the radiation material in terms of thickness

Table 3 e Effective atomic numbers of clay fly ash bricks.


Samples 661.6 keV 1,173.2 keV 1,332.5 keV
Experimental Theoretical Experimental Theoretical Experimental Theoretical
Clay 11.89 11.71 11.67 11.71 11.64 11.7
Fly ash 10.73 10.79 10.71 10.75 10.71 10.71
CF10 11.85 11.72 11.62 11.68 11.64 11.66
CF20 11.74 11.67 11.58 11.55 11.59 11.48
CF30 11.69 11.50 11.59 11.43 11.56 11.41
CF40 11.42 11.45 11.32 11.32 11.23 11.29
CF50 11.18 11.22 10.92 11.21 10.74 11.07

CF10, 10% fly ash content; CF20, 20% fly ash content; CF30, 30% fly ash content; CF40, 40% fly ash content; CF50, 50% fly ash content.

Table 4 e Electron densities (£ 1023 electrons/g) of clay fly ash bricks.


Samples 661.6 keV 1173.2 keV 1,332.5 keV
Experimental Theoretical Experimental Theoretical Experimental Theoretical
Clay 3.02 2.97 2.98 2.96 2.95 2.98
Fly ash 2.95 2.96 2.95 2.97 2.95 2.94
CF10 3.02 2.97 2.97 2.96 2.95 2.95
CF20 3.01 2.97 2.97 2.96 2.95 2.94
CF30 3.01 2.97 2.97 2.96 2.95 2.94
CF40 2.98 2.96 2.97 2.96 2.95 2.94
CF50 2.98 2.96 2.97 2.96 2.95 2.93

CF10, 10% fly ash content; CF20, 20% fly ash content; CF30, 30% fly ash content; CF40, 40% fly ash content; CF50, 50% fly ash content.
N u c l e a r E n g i n e e r i n g a n d T e c h n o l o g y 4 8 ( 2 0 1 6 ) 1 2 3 0 e1 2 3 6 1235

capability to gamma radiations. The gradual increase in HVL


Table 5 e The absorption % efficiency (approximate) of
of clay fly ash bricks from clay bricks is a maximum of 24% for
samples for gamma ray.
a 50/50 composition. It seems to be on the higher side due to
Samples Energy (keV)
the incorporation of low density fly ash, indicating the need
661.6 1173.2 1,332.5 for thicker clay fly ash bricks to shield against gamma radia-
Clay 95.6 91.1 89.7 tion in comparison to concrete. But this is of little significance
CF10 95.1 90.4 89.0 where space is not a constraint.
CF20 94.6 89.0 87.4
CF30 94.2 87.9 86.5
CF40 93.8 87.1 85.5
CF50 93.1 86.2 84.1
5. Conclusions
Concrete 95.9 94.1 92.4

CF10, 10% fly ash content; CF20, 20% fly ash content; CF30, 30% fly The shielding parameters of clay fly ash bricks for various
ash content; CF40, 40% fly ash content; CF50, 50% fly ash content.
compositions, in terms of percentage of fly ash in clay, used as
a building material in India were evaluated to obtain an
optimal composition mixture. This study concludes that, in
requirements. The increase in low density fly ash content in case of any nuclear accident, the good absorption efficiency of
bricks increases HVL, thus the shielding effectiveness is found multilayered exterior walls made of clay fly ash bricks can be
to be lower than that of concrete. used as a biological shield against low energy gamma rays.
Using the mass attenuation coefficients, the values of the These bricks can replace pure clay bricks, where space is not a
effective atomic numbers Zeff have been calculated on the constraint. Even the valuable clay, i.e., irreplaceable economic
basis of the mixture rule as shown in Table 3. The value of the resource can be conserved to the extent of 50% by weight. The
effective atomic number of samples is more or less constant study makes it clear that clay fly ash bricks can be beneficial to
for all samples in the investigated energy range. The con- address the issues of radiation shielding, cost effectiveness,
stancy of Zeff is due to the fact that the clay and fly ash consist radioactive waste management, and the disposal of fly ash in
of elements of very close atomic numbers. Also, it is attributed a useful manner.
to the Compton scattering, which is dominant in this range of
energy. A companion parameter to the effective atomic
number, used for energy deposition by photons in biological Conflicts of interest
shielding is electron density. The electron density is nearly
constant for all brick samples in the range of 2.93e3.02  1023 All authors have no conflict of interest to declare.
electrons per unit gram of material as shown in Table 4.

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